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Article Dans Une Revue Organometallics Année : 2014

Assembly of Platinum Diimine Dithiolate Complexes onto Hydrogen-Terminated Silicon Surfaces

Résumé

The synthesis and structural characterization of the platinum diimine dithiolate complexes [Pt(R2bipy)(dmipi)] (dmipi = 4,5-dimercapto-l,3-dithiol-2-propargylimino and R = H, tBu) are described together with the X-ray crystal structure of the dithiolate proligand. These heteroleptic Pt complexes have been covalently bound to hydrogen-terminated silicon (100) surfaces using either a one-step or two-step procedure. The redox-active organometallic film modified surfaces were prepared from a hydrosilylation reaction at 90 °C of either the Pt complex bearing an ethyne terminal group or an ethyne-terminated dithiolate precursor followed by the subsequent anchoring of the Pt complex. Cyclic voltammetry measurements showed the presence of a single reversible one-electron-oxidation process corresponding to the oxidation of the complex into its radical cation species at 0.42 and 0.46 V vs SCE for the unsubstituted and tBu-substituted bipyridine dithiolate Pt complex-modified Si(100) surfaces, respectively. Such values compare well with those determined for the electroactive molecules in solution. Moreover, FTIR spectroscopy and X-ray photoelectron spectroscopy (XPS) measurements were consistent with the expected structure of grafted molecular chains and revealed a significant oxidation of the underlying silicon surface. Nevertheless, the one-step procedure was found to lead to redox-active films of density higher than those produced from the two-step procedure. From XPS data, the surface coverage was estimated at 0.10 and in the range 0.03–0.06 Pt complex per surface silicon atom for the one-step and two-step procedures, respectively.

Domaines

Chimie organique
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Dates et versions

hal-01151688 , version 1 (13-05-2015)

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Gilles Yzambart, Bruno Fabre, Thierry Roisnel, Vincent Dorcet, S. Ababou-Girard, et al.. Assembly of Platinum Diimine Dithiolate Complexes onto Hydrogen-Terminated Silicon Surfaces. Organometallics, 2014, 33 (18), pp.4766-4776. ⟨10.1021/om5000369⟩. ⟨hal-01151688⟩
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